This work presents the synthesis of platinum nanoparticles (Pt NPs) and their subsequent deposition on the nitrogen-doped carbon nanotubes, which have been directly grown on a carbon cloth (CNT-CC electrode). The CNT-CC electrode provides a fast electron-transfer path to the carbon cloth, resulting in energy-loss reduction and enhancing catalytic activity of Pt NPs. The N-dopants in CNT serve as the defect sites to enhance nucleation of Pt particles. The reduction of the Pt precursor salt was carried out in the ethylene glycol solution at an elevated temperature. In order to control the Pt NP size, the pH of the reaction solution was controlled by the addition of NaOH. Zeta potential measurements of the as-prepared sample indicate that a higher zeta potential results in a smaller particle size, due to a stronger electrostatic repulsion between NPs. This serves a powerful tool for size control of the Pt nanoparticle. The Pt NPs dispersed on the CNT-CC have an average size of 2.81 nm (Pt/CNT-CC) prepared using 15 mM NaOH, with high uniformity under electron microscopy. Cyclic voltammetry measurements of the electrocatalytic activity of the Pt/CNT-CC for methanol oxidation indicate that it exhibits excellent electrocatalytic activity and are ideal for direct methanol fuel cell applications.